Interfacial Catalysis Engineering of Solid Electrolyte Interphase Toward High‐Performance Batteries

Abstract The solid electrolyte interphase (SEI) is a crucial passivation layer that governs the electrochemical stability, cycling lifespan, and coulombic efficiency (CE) of different battery systems. Research has been extensively performed on electrolyte engineering and artificial design for robust SEI formation, while precise control of electrolyte decomposition dynamics is largely overlooked. Recently, interfacial catalysis has emerged as a promising strategy to guide SEI formation via modulating the electrolyte decomposition behaviors. The selective decomposition of anions in the electrolyte can be accelerated via introducing unique catalytic sites at the electrode‐electrolyte interface, which enables precise tuning of SEI composition, microstructure reconstruction, and functionality enhancement. This review timely and systematically summarizes recent progress in the interfacial catalysis engineering of SEI layers, with a focus on catalytic mechanisms, catalyst design principles, and representative applications in various anode systems (e.g., lithium metal anode, sodium metal anode, alloy anodes, and carbonaceous anodes).